Acid anion electrolyte effects on platinum for oxygen and hydrogen electrocatalysis

Kamat, Gaurav Ashish; Zamora Zeledón, José A.; Gunasooriya, G. Kalhara; Dull, Samuel M.; Perryman, Joseph T.; Nørskov, Jens K.; Stevens, Michaela Burke; Jaramillo, Thomas F.

doi:10.1038/s42004-022-00635-1

Title: Acid anion electrolyte effects on platinum for oxygen and hydrogen electrocatalysis

Journal Article · 18 February 2022 · Communications Chemistry

DOI: https://doi.org/10.1038/s42004-022-00635-1 · OSTI ID:1841467

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Stanford Univ., CA (United States); Stanford Univ., CA (United States). SUNCAT Center for Interface Science and Catalysis; SLAC National Accelerator Lab., Menlo Park, CA (United States); SLAC National Accelerator Laboratory, Stanford University
Stanford Univ., CA (United States); Stanford Univ., CA (United States). SUNCAT Center for Interface Science and Catalysis; SLAC National Accelerator Lab., Menlo Park, CA (United States)
Technical Univ. of Denmark, Lyngby (Denmark). Catalysis Theory Center

Platinum is an important material with applications in oxygen and hydrogen electrocatalysis. To better understand how its activity can be modulated through electrolyte effects in the double layer microenvironment, herein we investigate the effects of different acid anions on platinum for the oxygen reduction/evolution reaction (ORR/OER) and hydrogen evolution/oxidation reaction (HER/HOR) in pH 1 electrolytes. Experimentally, we see the ORR activity trend of HClO₄ > HNO₃ > H₂SO₄, and the OER activity trend of HClO₄ > HNO₃ ~ H₂SO₄. HER/HOR performance is similar across all three electrolytes. Notably, we demonstrate that ORR performance can be improved 4-fold in nitric acid compared to in sulfuric acid. Assessing the potential-dependent role of relative anion competitive adsorption with density functional theory, we calculate unfavorable adsorption on Pt(111) for all the anions at HER/HOR conditions while under ORR/OER conditions ClO$$^{-}_{4}$$ binds the weakest followed by NO$$^{-}_{3}$$ and SO$$^{2-}_{4}$$. Our combined experimental-theoretical work highlights the importance of understanding the role of anions across a large potential range and reveals nitrate-like electrolyte microenvironments as interesting possible sulfonate alternatives to mitigate the catalyst poisoning effects of polymer membranes/ionomers in electrochemical systems. These findings help inform rational design approaches to further enhance catalyst activity via microenvironment engineering.

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Research Organization:: SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States); SLAC National Accelerator Laboratory, Stanford University

Sponsoring Organization:: National Science Foundation (NSF); USDOE Office of Science (SC), Basic Energy Sciences (BES); USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences & Biosciences Division

Contributing Organization:: SUNCAT

Grant/Contract Number:: AC02-76SF00515

OSTI ID:: 1841467

Journal Information:: Communications Chemistry, Journal Name: Communications Chemistry Journal Issue: 1 Vol. 5; ISSN 2399-3669

Publisher:: Springer NatureCopyright Statement

Country of Publication:: United States

Language:: English

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Source Data for Acid Anion Electrolyte Effects on Platinum for Oxygen and Hydrogen Electrocatalysis Zamora Zeledon, Jose; Gunasooriya, Kasun Govini Thanthrige Kalhara; Stevens, Michaela Burke figshare https://doi.org/10.6084/m9.figshare.16679665.v1	dataset	January 2022

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Related Subjects

36 MATERIALS SCIENCE
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
42 ENGINEERING
77 NANOSCIENCE AND NANOTECHNOLOGY
acid electrolyte
chemical engineering
electrocatalysis
energy
hydrogen
microenvironment
oxygen
platinum

Data for the 'Acid Anion Electrolyte Effects on Platinum for Oxygen and Hydrogen Electrocatalysis' Gunasooriya, Kasun Govini Thanthrige Kalhara https://doi.org/10.11583/DTU.18277970 The current record is supplemented by this dataset	dataset	January 2022
Data for the 'Acid Anion Electrolyte Effects on Platinum for Oxygen and Hydrogen Electrocatalysis' Gunasooriya, Kasun Govini Thanthrige Kalhara https://doi.org/10.11583/dtu.18277970.v1 The current record is supplemented by this dataset	dataset	January 2022
Source Data for Acid Anion Electrolyte Effects on Platinum for Oxygen and Hydrogen Electrocatalysis Zamora Zeledon, Jose; Gunasooriya, Kasun Govini Thanthrige Kalhara; Stevens, Michaela Burke https://doi.org/10.6084/m9.figshare.16679665 The current record is supplemented by this dataset	dataset	January 2022

Title: Acid anion electrolyte effects on platinum for oxygen and hydrogen electrocatalysis

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